杂原子
溶解
法拉第效率
格式化
硫黄
催化作用
价(化学)
化学
密度泛函理论
硫化物
兴奋剂
电子结构
电化学
无机化学
材料科学
电极
物理化学
计算化学
有机化学
光电子学
戒指(化学)
作者
Fei Liu,Xixi Ren,Jianlin Zhao,Han Wu,Jiajun Wang,Xiaopeng Han,Yida Deng,Wenbin Hu
出处
期刊:ACS Catalysis
日期:2022-10-20
卷期号:12 (21): 13533-13541
被引量:21
标识
DOI:10.1021/acscatal.2c02617
摘要
Heteroatom doping can facilitate intrinsic activity via the tuning of electronic states. However, it is still rare to elucidate the role of a specific metal sulfide electronic state and simultaneously enhance the CO2 electroreduction reaction (CO2RR) stability. SnS is well-known for its ability to produce HCOOH; however, its long-term operational stability is limited by sulfur dissolution. Herein, we propose a strategy to reinforce the S atoms via heteroatom (In) doping. In situ Raman tests and theoretical calculations demonstrate that In atoms with fewer valence electrons (compared with Sn) can tune the electronic state of SnS and strengthen the S–metal bond energy. Consequently, sulfur dissolution was inhibited, and the reaction pathway was optimized. Further, the In-SnS/C achieves a Faradaic efficiency of 96.6% for formate at −0.6 V vs RHE and a catalyst stability of 50 h at a current density of ∼37 mA cm–2. This study shows that altering the electronic structure of SnS via heteroatoms is a strategy to optimize both the activity and stability of electrocatalysts for the CO2RR.
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